Electronic Interactions of Size-Selected Oxide Clusters on Metallic and Thin Film Oxide Supports
Abstract
The interfacial electronic structure of various size-selected metal oxide nanoclusters (M3Ox; M = Mo, Nb, Ti) on Cu(111) and a thin film of Cu2O supports were investigated in this paper by a combination of experimental methods and density functional theory (DFT). These systems explore electron transfer at the metal–metal oxide interface which can modify surface structure, metal oxidation states, and catalytic activity. Electron transfer was probed by measurements of surface dipoles derived from coverage dependent work function measurements using two-photon photoemission (2PPE) and metal core level binding energy spectra from X-ray photoelectron spectroscopy (XPS). The measured surface dipoles are negative for all clusters on Cu(111) and Cu2O/Cu(111), but those on the Cu2O surface are much larger in magnitude. In addition, sub-stoichiometric or “reduced” clusters exhibit smaller surface dipoles on both the Cu(111) and Cu2O surfaces. Negative surface dipoles for clusters on Cu(111) suggest Cu → cluster electron transfer, which is generally supported by DFT-calculated Bader charge distributions. For Cu2O/Cu(111), calculations of the surface electrostatic potentials show that the charge distributions associated with cluster adsorption structures or distortions at the cluster–Cu2O–Cu(111) interface are largely responsible for the observed negative surface dipoles. Changes observed in the XPS spectra for the Mo 3d,more »
- Authors:
-
[2];
[3]
- Stony Brook Univ., NY (United States). Dept. of Chemistry
- Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
- Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.; Stony Brook Univ., NY (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1412738
- Report Number(s):
- BNL-114561-2017-JA
Journal ID: ISSN 1932-7447; R&D Project: CO007; KC0301020; TRN: US1800337
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 121; Journal Issue: 40; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Xue, Meng, Nakayama, Miki, Liu, Ping, and White, Michael G. Electronic Interactions of Size-Selected Oxide Clusters on Metallic and Thin Film Oxide Supports. United States: N. p., 2017.
Web. doi:10.1021/acs.jpcc.7b07889.
Xue, Meng, Nakayama, Miki, Liu, Ping, & White, Michael G. Electronic Interactions of Size-Selected Oxide Clusters on Metallic and Thin Film Oxide Supports. United States. https://doi.org/10.1021/acs.jpcc.7b07889
Xue, Meng, Nakayama, Miki, Liu, Ping, and White, Michael G. Wed .
"Electronic Interactions of Size-Selected Oxide Clusters on Metallic and Thin Film Oxide Supports". United States. https://doi.org/10.1021/acs.jpcc.7b07889. https://www.osti.gov/servlets/purl/1412738.
@article{osti_1412738,
title = {Electronic Interactions of Size-Selected Oxide Clusters on Metallic and Thin Film Oxide Supports},
author = {Xue, Meng and Nakayama, Miki and Liu, Ping and White, Michael G.},
abstractNote = {The interfacial electronic structure of various size-selected metal oxide nanoclusters (M3Ox; M = Mo, Nb, Ti) on Cu(111) and a thin film of Cu2O supports were investigated in this paper by a combination of experimental methods and density functional theory (DFT). These systems explore electron transfer at the metal–metal oxide interface which can modify surface structure, metal oxidation states, and catalytic activity. Electron transfer was probed by measurements of surface dipoles derived from coverage dependent work function measurements using two-photon photoemission (2PPE) and metal core level binding energy spectra from X-ray photoelectron spectroscopy (XPS). The measured surface dipoles are negative for all clusters on Cu(111) and Cu2O/Cu(111), but those on the Cu2O surface are much larger in magnitude. In addition, sub-stoichiometric or “reduced” clusters exhibit smaller surface dipoles on both the Cu(111) and Cu2O surfaces. Negative surface dipoles for clusters on Cu(111) suggest Cu → cluster electron transfer, which is generally supported by DFT-calculated Bader charge distributions. For Cu2O/Cu(111), calculations of the surface electrostatic potentials show that the charge distributions associated with cluster adsorption structures or distortions at the cluster–Cu2O–Cu(111) interface are largely responsible for the observed negative surface dipoles. Changes observed in the XPS spectra for the Mo 3d, Nb 3d, and Ti 2p core levels of the clusters on Cu(111) and Cu2O/Cu(111) are interpreted with help from the calculated Bader charges and cluster adsorption structures, the latter providing information about the presence of inequivalent cation sites. Finally, the results presented in this work illustrate how the combined use of different experimental probes along with theoretical calculations can result in a more realistic picture of cluster–support interactions and bonding.},
doi = {10.1021/acs.jpcc.7b07889},
journal = {Journal of Physical Chemistry. C},
number = 40,
volume = 121,
place = {United States},
year = {Wed Sep 13 00:00:00 EDT 2017},
month = {Wed Sep 13 00:00:00 EDT 2017}
}
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